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Expectation values of physical quantities may accurately be obtained by the evaluation of integrals within Many-Body Quantum mechanics, and these multi-dimensional integrals may be estimated using Monte Carlo methods. In a previous…

Computational Physics · Physics 2009-10-01 J. R. Trail

The ground and excited state calculations at key geometries, such as the Frank-Condon (FC) and the conical intersection (CI) geometries, are essential for understanding photophysical properties. To compute these geometries on noisy…

Quantum Physics · Physics 2023-01-02 Shigeki Gocho , Hajime Nakamura , Shu Kanno , Qi Gao , Takao Kobayashi , Taichi Inagaki , Miho Hatanaka

The essence of atomic structure theory, quantum chemistry, and computational materials science is solving the multi-electron stationary Schr\"odinger equation. The Quantum Monte Carlo-based neural network wave function method has surpassed…

Atomic Physics · Physics 2023-12-27 JinDe Liu , Chenglong Qin , Xi He , Gang Jiang

Quantum Monte Carlo (QMC) methods have proven to be highly accurate for computing excited states, but the choice of optimization strategies for multiple states remains an active topic of investigation. In this work, we revisit the…

Computational Physics · Physics 2025-04-15 Stuart Shepard , Anthony Scemama , Saverio Moroni , Claudia Filippi

We propose a new variational Monte Carlo (VMC) method with an energy variance extrapolation for large-scale shell-model calculations. This variational Monte Carlo is a stochastic optimization method with a projected correlated condensed…

Nuclear Theory · Physics 2012-02-14 Takahiro Mizusaki , Noritaka Shimizu

Solutions to many-body problem instances often involve an intractable number of degrees of freedom and admit no known approximations in general form. In practice, representing quantum-mechanical states of a given Hamiltonian using available…

Quantum Physics · Physics 2020-11-10 Andrey Kardashin , Alexey Uvarov , Dmitry Yudin , Jacob Biamonte

Variational wave functions used in the variational Monte Carlo (VMC) method are extensively improved to overcome the biases coming from the assumed variational form of the wave functions. We construct a highly generalized variational form…

Strongly Correlated Electrons · Physics 2008-10-27 Daisuke Tahara , Masatoshi Imada

We present and motivate an efficient way to include orbital dependent many--body correlations in trial wave function of real--space Quantum Monte Carlo methods for use in electronic structure calculations. We apply our new…

Computational Physics · Physics 2019-10-17 Markus Holzmann , Saverio Moroni

We combine recent advances in excited state variational principles, fast multi-Slater Jastrow methods, and selective configuration interaction to create multi-Slater Jastrow wave function approximations that are optimized for individual…

Strongly Correlated Electrons · Physics 2019-06-19 Sergio D. Pineda Flores , Eric Neuscamman

Ab initio quantum Monte Carlo (QMC) is a state-of-the-art numerical approach for evaluating accurate expectation values of many-body wavefunctions. However, one of the major drawbacks that still hinders widespread QMC applications is the…

Materials Science · Physics 2024-07-17 Kousuke Nakano , Michele Casula , Giacomo Tenti

We employ a generalized variational principle to improve the stability, reliability, and precision of fully excited-state-specific complete active space self-consistent field theory. Compared to previous approaches that similarly seek to…

Chemical Physics · Physics 2022-09-05 Rebecca Hanscam , Eric Neuscamman

We present a new approach to calculate excited states with the full configuration interaction quantum Monte Carlo (FCIQMC) method. The approach uses a Gram-Schmidt procedure, instantaneously applied to the stochastically evolving…

Computational Physics · Physics 2015-10-28 N. S. Blunt , Simon D. Smart , George H. Booth , Ali Alavi

We present a novel specialization of the variational Monte Carlo linear method for the optimization of the recently introduced cluster Jastrow antisymmetric geminal power ansatz, achieving a lower-order polynomial cost scaling than would be…

Chemical Physics · Physics 2016-03-23 Eric Neuscamman

The calculation of excited state energies of electronic structure Hamiltonians has many important applications, such as the calculation of optical spectra and reaction rates. While low-depth quantum algorithms, such as the variational…

Quantum Physics · Physics 2019-07-03 Oscar Higgott , Daochen Wang , Stephen Brierley

A variational approach is used to calculate free energy and conformational properties in polyelectrolytes. The true bond and Coulomb potentials are approximated by a trial isotropic harmonic energy containing monomer-monomer force constants…

High Energy Physics - Lattice · Physics 2009-09-25 B. Jönsson , C. Peterson , B. Söderberg

Variational methods have proven to be excellent tools to approximate ground states of complex many body Hamiltonians. Generic tools like neural networks are extremely powerful, but their parameters are not necessarily physically motivated.…

Strongly Correlated Electrons · Physics 2022-03-04 Agnes Valenti , Eliska Greplova , Netanel H. Lindner , Sebastian D. Huber

A recently developed self-healing diffusion Monte Carlo algorithm [PRB 79, 195117] is extended to the calculation of excited states. The formalism is based on an excited-state fixed-node approximation and the mixed estimator of the…

Strongly Correlated Electrons · Physics 2015-05-13 Fernando A. Reboredo

We present high-accuracy correlated calculations of small Si$_x$H$_y$ molecular systems both in the ground and excited states. We employ quantum Monte Carlo (QMC) together with a variety of many-body wave function approaches based on basis…

Chemical Physics · Physics 2020-10-21 Guangming Wang , Abdulgani Annaberdiyev , Lubos Mitas

This study explores the application of neural network variational Monte Carlo (NN-VMC) for the computation of low-lying excited states in molecular systems. Our focus lies on the implementation and evaluation of two distinct methodologies,…

Computational Physics · Physics 2023-11-30 Zixiang Lu , Weizhong Fu

We investigate two kinds of extensions for the variational Monte Carlo (VMC) method with the Pfaffian in the nuclear shell-model calculations. One is the extension to odd-mass nuclei, for which we find a new Pfaffian expression of the VMC…

Nuclear Theory · Physics 2018-11-21 Noritaka Shimizu , Takahiro Mizusaki